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Redox-Controlled Shunts in a Synthetic Chemical Reaction Cycle

[Image: see text] Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enabl...

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Detalles Bibliográficos
Autores principales: Sharko, Anastasiia, Spitzbarth, Benjamin, Hermans, Thomas M., Eelkema, Rienk
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10161229/
https://www.ncbi.nlm.nih.gov/pubmed/37092741
http://dx.doi.org/10.1021/jacs.3c00985
Descripción
Sumario:[Image: see text] Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enable access to two shunts within this CRN with different kinetics and a reduced number of side reactions compared to the main cycle that is driven by strong oxidants. Furthermore, we introduce a strategy to recycle one of the main products under flow conditions to partially reverse the CRN and control product speciation throughout time. These findings introduce new levels of control over artificial CRNs, driven by redox chemistry, narrowing the gap between synthetic and natural systems.